We experimentally studied the Rydberg level shift caused by the electric field, which is generated by Rydberg atom collision induced ionization in a cesium atomic ensemble. The density of charged particles caused by collisions between Rydberg atoms is changed by controlling the ground-state atomic density and optical excitation process. We measured the Rydberg level shift using Rydberg electromagnetically-induced-transparency (EIT) spectroscopy, and interpreted the physical origin using a semi-classical model. The experimental results are in good agreement with the numerical simulation. These energy shifts are important for the self-calibrated sensing of microwave field by the employing of Rydberg EIT. Moreover, in contrast to the resonant excitation case, narrow-linewidth spectroscopy with high signal-to-noise ratio would be useful for high-precision measurements.
Long ground-Rydberg coherence lifetime is interesting for implementing high-fidelity quantum logic gates, many-body physics, and other quantum information protocols. However, the potential formed by a conventional far-off-resonance red-detuned optical-dipole trap (ODT) is usually repulsive for Rydberg atoms, which will result in fast atom loss and low repetition rate of the experimental sequence. These issues can be addressed by a magic ODT. We performed the calculation of ODT's magic detuning for confinement of cesium ground state and Rydberg state with the same potential well. We used a sum-…
Cold Rydberg atoms subject to long-range dipole-dipole interactions represent a particularly interesting system for exploring few-body interactions and probing the transition from 2-body physics to the many-body regime. In this work we report the direct observation of a resonant 4-body Rydberg interaction. We exploit the occurrence of an accidental quasi-coincidence of a 2-body and a 4-body resonant Stark-tuned Forster process in cesium to observe a resonant energy transfer requiring the simultaneous interaction of at least four neighboring atoms. These results are relevant for the implementat…
Electrostatic multipole interactions generate long-range Rydberg-Rydberg macrodimer. We calculate the adiabatic potentials of cesium $(nD_{J})_2$ Rydberg macrodimers for principal quantum numbers $n$ ranging from 56 to 62, for $J=3/2$ and $5/2$, and for the allowed values of the conserved sum of the atomic angular-momentum components along the internuclear axis, $M$. For most combinations $(n, M, J)$ exactly one binding potential exists, which should give rise to Rydberg macrodimer states. We study the dependence of the adiabatic potentials on the size of the two-body basis sets used in the ca…
We experimentally investigate trap-loss spectra of the cesium 6S1/2(F=4)-71P3/2 Rydberg state by combining the cesium atomic magneto-optical trap with the narrow-linewidth, continuously-tunable 318.6 nm ultraviolet laser. That is, the atoms in the magneto-optical trap are excited to the Rydberg state due to the ultraviolet laser single-step Rydberg excitation, which leads to the reduction of atomic fluorescence. Based on the trap-loss spectroscopy technology, the Autler-Townes splitting due to strong cooling laser is observed, and the parameter dependence of the AT splitting interval of trap-l…
We study Rydberg atoms modulated by strong radio-frequency (RF) fields with a frequency of 70 MHz. The Rydberg atoms are prepared in a room temperature cesium cell, and their level structure is probed using electromagnetically induced transparency (EIT). As the RF field increases from the weak- into the strong-field regime, the range of observed RF-induced phenomena progresses from AC level shifts through increasingly pronounced and numerous RF-modulation sidebands to complex state-mixing and level-crossings with high-l hydrogen-like states. Weak anharmonic admixtures in the RF field generate …
We demonstrate the single-photon excitation spectra of cesium Rydberg atoms by means of a Doppler-free purely all-optical detection with a room-temperature vapor cell and a 319 nm ultra-violet (UV) laser. We excite atoms directly from 6S1/2 ground state to 71P3/2 Rydberg state with a narrow-linewidth 319 nm UV laser. The detection of Rydberg states is performed by monitoring the absorption of an 852 nm probe beam in a V-type three-level system. With a strong coupling light, we observe the Autler-Townes doublet and investigate experimentally the dependence of the separation and linewidth on the…
We report on the observation of electromagnetically induced transparency (EIT) and absorption (EIA) of highly excited Rydberg states in thermal Cs vapor using a four-step excitation scheme. The advantage of this four-step scheme is that the final transition to the Rydberg state has a large dipole moment and one can achieve similar Rabi frequencies to two- or three-step excitation schemes using two orders of magnitude less laser power. This scheme enables new applications such as dephasing free Rydberg excitation. The observed lineshapes are in good agreement with simulations based on multileve…
We demonstrate the single-photon Rydberg excitation of cesium atoms in a magneto-optical trap (MOT). We excite atoms directly from ${{6S}_{1/2}}$ ground state to ${{nP}_{3/2}}(n=70-100)$ Rydberg state with a narrow-linewidth 319 nm ultra-violet laser. The detection of Rydberg states is performed by monitoring the reduction of fluorescence signal of the MOT as partial population on ${{6S}_{1/2}} (F = 4)$ ground state are transferred to Rydberg state. We clearly observe Autler-Townes doublet in the trap-loss spectra due to the cooling lights. Utilizing the large electric polarizibility of Rydber…
Long-range macrodimers formed by D-state cesium Rydberg atoms are studied in experiments and in calculations. Cesium 62DJ-62DJ Rydberg-atom macrodimers, bonded via long-range multipole interaction, are prepared by two-color photo-association in a cesium atom trap. The first color (pulse A) resonantly excites seed Rydberg atoms, while the second (pulse B, detuned by the molecular binding energy) resonantly excites the Rydberg-atom macrodimer states below the 62DJ pair asymptotes. The Rydberg-atom molecules are measured by extraction of auto-ionization products and Rydberg-atom electric-field io…
We study Rydberg electromagnetically induced transparency (EIT) of a cascade three-level atom involving 80$D_{5/2}$ state in a strong interaction regime employing a cesium ultracold cloud. In our experiment, a strong coupling laser couples 6$P_{3/2}$ to 80$D_{5/2}$ transition, while a weak probe, driving 6$S_{1/2}$ to 6$P_{3/2}$ transition, probes the coupling induced EIT signal. At the two-photon resonance, we observe that the EIT transmission decreases slowly with time, which is a signature of interaction induced metastability. The dephasing rate $γ_{\rm OD}$ is extracted with optical depth …
We demonstrate a single-photon Rydberg excitation spectroscopy of cesium (Cs) atoms in a room-temperature vapor cell. Cs atoms are excited directly from 6S1/2 ground state to nP3/2 (n = 70 - 100) Rydberg states with a 318.6 nm ultraviolet (UV) laser,and Rydberg excitation spectra are obtained by transmission enhancement of a probe beam resonant to Cs 6S1/2, F = 4 - 6P3/2, F' = 5 transition as partial population on F = 4 ground state are transferred to Rydberg state .Analysis reveals that the observed spectra are velocity-selective spectroscopy of Rydberg state, from which the amplitude and lin…
We investigate the phenomenon of optical bistability in a driven ensemble of Rydberg atoms. By performing two experiments with thermal vapors of rubidium and cesium, we are able to shed light onto the underlying interaction mechanisms causing such a non-linear behavior. Due to the different properties of these two atomic species, we conclude that the large polarizability of Rydberg states in combination with electric fields of spontaneously ionized Rydberg atoms is the relevant interaction mechanism. In the case of rubidium, we directly measure the electric field in a bistable situation via tw…
Three body resonant interactions between Rydberg atoms are considered in order to perform few-body quantum gates. So far, the resonances found in cesium or rubidium atoms relied on an adjacent two-body resonance which ceases to exist for principal quantum numbers above $n \simeq 40$. We have proposed recently a new class of 3-body interaction resonances in alkali-metal Rydberg atoms [P. Cheinet \textit{et al.}, Quant. Elect. \textbf{50}, 213 (2020)], which circumvienes this limit. We investigate here the relative strength between this new class of 3-body interaction resonance and quasi-forbidd…
We report clear evidence of the role of dipole-dipole interaction in Penning ionization of Rydberg atoms, leading to the formation of an ultracold plasma. Penning ionization of np Rydberg Cesium atoms is prevented for states with in n < 42, which correspond to a repulsive potential, but it does not occur for n larger than 42, corresponding to an attractive potential. Blackbody radiation is mostly responsible for the background and initial ionization, although ion-Rydberg collisions and population transfer due to limited superradiance may have to be considered.
We study the field-ionization threshold behavior when a Rydberg atom is ionized by a short single-cycle pulse field. Both hydrogen and sodium atoms are considered. The required threshold field amplitude is found to scale \emph{inversely} with the binding energy when the pulse duration becomes shorter than the classical Rydberg period, and, thus, more weakly bound electrons require larger fields for ionization. This threshold scaling behavior is confirmed by both 3D classical trajectory Monte Carlo simulations and numerically solving the time-dependent Schrödinger equation. More surprisingly, t…
The phase noise of incident light fields can be converted into amplitude noise via absorption and dispersion effects in media under electromagnetically induced transparency. The conversion process is sensitive to two-photon detuning. This effect can be used to perform a novel type of Rydberg spectroscopy. We present experimental measurements of the phase noise spectrum (PNS) with Rydberg atoms in a cesium vapor cell. Furthermore, to explore microwave field measurements, a modulation-enhanced PNS approach is proposed.
The results of a theoretical investigation of prompt many-body ionization are reported. Our calculations address an experiment that reported ionization in Rydberg gases for densities two orders of magnitude less than expected from ionization between pairs of atoms. The authors argued that the results were due to the simultaneous interaction between many atoms. We performed classical calculations for many interacting Rydberg atoms with the ions fixed in space and have found that the many atom interaction does allow ionization at lower densities than estimates from two atom interactions. However…
A fully classical explanation of the nonhydrogenic ionization threshold for low angular momentum Rydberg states of Alkali-metal atoms in a linearly polarized low frequency monochromatic microwave field is given: the classical equivalent to the quantum rate-limiting step, which is responsible for the n^(-5) scaling and which according to the literature initiates what then continues as essentially classical diffusion, is found.
Collisional ionization between two Rydberg atoms in relative motion is examined. A classical trajectory Monte Carlo method is used to determine the cross sections associated with Penning ionization. The dependence of the ionization cross section on the magnitude and the direction of orbital angular momentum of the electrons and the direction of the Laplace-Runge-Lenz vector of the electrons is studied. For a given magnitude of angular momentum, there can exist a difference of a factor of up to $\sim2.5$ in the ionization cross section between the orientation with the highest and the lowest ion…
Tunnel ionization rates of triplet Rydberg states in helium with principal quantum numbers close to 37 have been measured in electric fields at the classical ionization threshold of $\sim197$ V/cm. The measurements were performed in the time domain by combining high-resolution continuous-wave laser photoexcitation and pulsed electric field ionization. The observed tunnel ionization rates range from $10^5$ s$^{-1}$ to $10^7$ s$^{-1}$ and have, together with the measured atomic energy-level structure in the corresponding electric fields, been compared to the results of calculations of the eigenv…
We report on the observation and numerical calculation of ionization spectra of highly Stark-shifted Rydberg states of rubidium beyond the classical ionization threshold. In the numerical calculations, a complex absorbing potential (CAP) allows us to predict the energy levels and ionization rates of Rydberg states in this regime. Our approach of adjusting the CAP to the external electric field reduces the number of free parameters from one per resonance to a single one. Furthermore, we have measured the ionization spectra of magneto-optically trapped rubidium atoms which are excited to princip…
We present an experimental and theoretical study of the chaotic ionization of quasi-one-dimensional potassium Rydberg wavepackets via a phase-space turnstile mechanism. Turnstiles form a general transport mechanism for numerous chaotic systems, and this study explicitly illuminates their relevance to atomic ionization. We create time-dependent Rydberg wavepackets, subject them to alternating applied electric-field "kicks", and measure the electron survival probability. Ionization depends not only on the initial electron energy, but also on the phase-space position of the electron with respect …
New experimental quantum simulation platforms have recently been implemented with divalent atoms trapped in optical tweezer arrays with promising performance. The second valence electron also brings new propects through the so-called Isolated Core Excitation (ICE), however autoionization presents a strong limitation to this use. In this study, we propose and demonstrate a new approach to applying a sizable light shift to a Rydberg state with close-to-resonant ICE while avoiding auto-ionization. In particular, we have investigated ICE of ytterbium atoms in $^1S_0$ Rydberg states. Spectroscopic …
Quantum control of the pathway along which a Rydberg electron field ionizes is experimentally and computationally demonstrated. Selective field ionization is typically done with a slowly rising electric field pulse. The $(1/n^*)^4$ scaling of the classical ionization threshold leads to a rough mapping between arrival time of the electron signal and principal quantum number of the Rydberg electron. This is complicated by the many avoided level crossings that the electron must traverse on the way to ionization, which in general leads to broadening of the time-resolved field ionization signal. In…
Coupling by the resonant dipole-dipole energy transfer between cold cesium Rydberg atoms is investigated using time-resolved narrow-band de-excitation spectroscopy. This technique combines the advantage of efficient Rydberg excitation with high-resolution spectroscopy at variable interaction times. The coherent character of the process is studied by back and forth transfer in the np+np <--> ns+(n+1)s reaction. Decoherence in the ensemble has two different origins: the atom motion induced by dipole-dipole interaction and the migration of the s-Rydberg excitation in the environment of p-Rydberg …
It is well-known from numerical and experimental results that the fraction of Rydberg states (excited neutral atoms) created by tunnel ionization declines dramatically with increasing ellipticity of laser light. We present a method to analyze this dependence on ellipticity, deriving a probability distribution of Rydberg states that agrees closely with recent experimental [1] and numerical results. In particular, contradicting the existing proposed mechanism [1] and general expectations, our results indicate that the dependence of Rydberg yield on laser ellipticity is not caused by a rescatteri…
High resolution laser Stark excitation of np (60 < n < 85) Rydberg states of ultra-cold cesium atoms shows an efficient blockade of the excitation attributed to long-range dipole-dipole interaction. The dipole blockade effect is observed as a quenching of the Rydberg excitation depending on the value of the dipole moment induced by the external electric field. Effects of eventual ions which could match the dipole blockade effect are discussed in detail but are ruled out for our experimental conditions. Analytic and Monte-Carlo simulations of the excitation of an ensemble of interacting Rydberg…
High resolution laser excitation of np Rydberg states of cesium atoms shows a dipole blockade at Förster resonances corresponding to the resonant dipole-dipole energy transfer of the np + np → ns + (n + 1)s reaction. The dipole-dipole interaction can be tuned on and off by the Stark effect, and such a process observed for relatively low n (25 − 41) is promising for quantum gate devices. Both Penning ionization and saturation in the laser excitation can limit the range of observation of the dipole blockade
Pulsed field ionization of high-$n$ (90 $\leq n \leq$ 150) manifold states in Rb Rydberg atoms has been investigated in high slew-rate regime. Two peaks in the field ionization spectra were systematically observed for the investigated $n$ region, where the field values at the lower peak do not almost depend on the excitation energy in the manifold, while those at the higher peak increase with increasing excitation energy. The fraction of the higher peak component to the total ionization signals increases with increasing $n$, exceeding 80% at $n$ = 147. Characteristic behavior of the peak compo…
We have developed a quite stringent method in selectivity to ionize the low angular- momentum ($\ell$) states which lie below and above the adjacent manifold in highly excited Rb Rydberg atoms. The method fully exploits the pulsed field-ionization characteristics of the manifold states in high slew-rate regime: Specifically the low $\ell$ state below (above) the adjacent manifold is firstly transferred to the lowest (highest) state in the manifold via the adiabatic transition at the first avoided crossing in low slew-rate regime, and then the atoms are driven to a high electric field for ioniz…
Multi-step laser resonance ionization spectroscopy of lutetium (Lu) has been performed at TRIUMF's off-line laser ion source test stand. The even-parity Rydberg series $6s^2nd$ $^2D_{3/2}$, $6s^2nd$ $^2D_{5/2}$ and $6s^2ns$ $^2S_{1/2}$ were observed converging to the 6s$^2$ ionization potential. The experimental results has been compared to previous work. 51 levels of Rydberg series $6s^2nd$ $^2D_{5/2}$ and 52 levels of Rydberg series $6s^2ns$ $^2S_{1/2}$ were reported new. Additionally six even-parity autoionization (AI) series converging to Lu ionic states $5d6s$ $^3D_1$ and $5d6s$ $^3D_2$ w…
I show that the theory developed for quantum delocalization of an excited Hydrogen atom in a two-frequency linearly polarized microwave field can be used with a few adaptions to explain the quantum delocalization of Alkali atoms in a linearly polarized monochromatic field in the regime where it deviates from Hydrogenic behaviour. Comparison with numerical and laboratory experiments is satisfactory: apart from a constant factor, independent from the microwave frequency, the same dependence from the initial quantum number is observed.
We present a new mechanism contributing to the detection of photoassociated long-range Rydberg molecules via pulsed-field ionization: ionic products, created by the decay of a long-range Rydberg molecule, modify the excitation spectrum of surrounding ground-state atoms and facilitate the excitation of further atoms into Rydberg states by the photoassociation light. Such an ion-mediated excitation mechanism has been previously called "Coulomb anti-blockade". Pulsed-field ionisation typically doesn't discriminate between the ionization of a long-range Rydberg molecule and an isolated Rydberg ato…
We report new frequency-comb-based measurements of Ca Rydberg energy levels. Counter-propagating laser beams at 390 nm and 423 nm excite Ca atoms from the $4s^2~^1\mbox{S}_0$ ground state to $4sns~^1\mbox{S}_0$ Rydberg levels with $n$ ranging from 40 to 110. Near-resonant two-photon two-color excitation of atoms in a thermal beam makes it possible to eliminate the first-order Doppler shift. The resulting lineshapes are symmetric and Gaussian. We verify laser metrology and absolute accuracy by reproducing measurements of well-known transitions in Cs, close to the fundamental wavelengths of our …
We present time-resolved spectroscopic measurements of Rydberg-Rydberg interactions in an ultracold gas, revealing the pair dynamics induced by long-range van der Waals interactions between the atoms. By detuning the excitation laser, a specific pair distribution is prepared. Penning ionization on a microsecond timescale serves as a probe for the pair dynamics under the influence of the attractive long-range forces. Comparison with a Monte Carlo model not only explains all spectroscopic features but also gives quantitative information about the interaction potentials. The results imply that th…
Coherent time evolution of highly excited Rydberg states in Rb (98 < n < 150) under pulsed electric field in high slew-rate regime was investigated with the field ionization detection. The electric field necessary to ionize the Rydberg states was found to take discrete values successively depending on the slew rate. Specifically the slew-rate dependence of the ionization field varies with the quantum defect value of the states, i.e. with the energy position of the states relative to the adjacent manifold. This discrete transitional behavior of the ionization field observed for the first time i…
This work reports on the application of a novel electric field-ionization setup for high-resolution laser spectroscopy measurements on bunched fast atomic beams in a collinear geometry. In combination with multi-step resonant excitation to Rydberg states using pulsed lasers, the field ionization technique demonstrates increased sensitivity for isotope separation and measurement of atomic parameters over non-resonant laser ionization methods. The setup was tested at the Collinear Resonance Ionization Spectroscopy experiment at ISOLDE-CERN to perform high-resolution measurements of transitions i…
Long-range metastable molecules consisting of two cesium atoms in high Rydberg states have been observed in an ultracold gas. A sequential three-photon two-color photoassociation scheme was employed to form these molecules in states which correlate to $np(n+1)s$ dissociation asymptotes. Spectral signatures of bound molecular states are clearly resolved at the positions of avoided crossings between long-range van der Waals potential curves. The experimental results are in agreement with simulations based on a detailed model of the long-range multipole-multipole interactions of Rydberg-atom pair…
We investigate a possible mechanism for the autoionization of ultracold Rydberg gases, based on the resonant coupling of Rydberg pair states to the ionization continuum. Unlike an atomic collision where the wave functions begin to overlap, the mechanism considered here involves only the long-range dipole interaction and is in principle possible in a static system. It is related to the process of intermolecular Coulombic decay (ICD). In addition, we include the interaction-induced motion of the atoms and the effect of multi-particle systems in this work. We find that the probability for this io…
The electron signals from the field ionization of two closely-spaced Rydberg states of \mbox{rubidium-85} are separated using quantum control. In selective field ionization, the state distribution of a collection of Rydberg atoms is measured by ionizing the atoms with a ramped electric field. Generally, atoms in higher energy states ionize at lower fields, so ionized electrons which are detected earlier in time can be correlated with higher energy Rydberg states. However, the resolution of this technique is limited by the Stark effect. As the electric field is increased, the electron encounter…
We investigate the phenomenon of bistability in a thermal gas of cesium atoms excited to Rydberg states. We present both measurements and a numerical model of the phenomena based on collisions. By directly measuring the plasma frequency, we show that the origin of the bistable behavior lies in the creation of a plasma formed by ionized Rydberg atoms. Recombination of ions and electrons manifests as fluorescence which allows us to characterize the plasma properties and study the transient dynamics of the hysteresis that occurs. We determine scaling parameters for the point of plasma formation, …
We have studied an ionization of alkali-metal Rydberg atoms by blackbody radiation (BBR). The results of the theoretical calculations of ionization rates of Li, Na, K, Rb and Cs Rydberg atoms are presented. Calculations have been performed for nS, nP and nD states which are commonly used in a variety of experiments, at principal quantum numbers n=8-65 and at the three ambient temperatures of 77, 300 and 600 K. A peculiarity of our calculations is that we take into account the contributions of BBR-induced redistribution of population between Rydberg states prior to photoionization and field ion…
The passage of cold cesium 49S$_{1/2}$ Rydberg atoms through an electric-field-induced multi-level avoided crossing with nearby hydrogen-like Rydberg levels is employed to prepare a cold, dipolar Rydberg atom gas. When the electric field is ramped through the avoided crossing on time scales on the order of 100~ns or slower, the 49S$_{1/2}$ population adiabatically transitions into high-\emph{l} Rydberg Stark states. The adiabatic state transformation results in a cold gas of Rydberg atoms with large electric dipole moments. After a waiting time of about $1~μ$s and at sufficient atom density, t…
Rydberg atoms have shown significant promise as the basis for highly sensitive detectors of continuous radio-frequency (RF) E-fields. Here, we study their time-dependent response to pulse-modulated RF E-fields at 19.4 GHz using a cesium vapour cell at room temperature. We use density matrix simulations to explain the time scales that shape the transient atomic response under different laser conditions, finding them to be limited by dephasing mechanisms including transit time broadening, Rydberg-Rydberg collisions, and ionization. Using a matched filter, we demonstrate the detection of individu…
We observe that when an ultracold ground state cesium (Cs) atom becomes bound within the electronic cloud of an extended Cs electronic orbit, ultralong-range molecules with giant (kilo-Debye) permanent electric dipole moments form. Large molecular permanent electric dipole moments are challenging to experimentally realize. Meeting this challenge has garnered significant interest because permanent electric dipole moments are important for understanding symmetry breaking in molecular physics, control of chemical reactions and realization of strongly correlated many-body quantum systems. These ne…
We characterized the pulsed Rydberg-positronium production inside the AEgIS (Antimatter Experiment: Gravity, Interferometry, Spectroscopy) apparatus in view of antihydrogen formation by means of a charge exchange reaction between cold antiprotons and slow Rydberg-positronium atoms. Velocity measurements on positronium along two axes in a cryogenic environment (10K) and in 1T magnetic field were performed. The velocimetry was done by MCP-imaging of photoionized positronium previously excited to the $n=3$ state. One direction of velocity was measured via Doppler-scan of this $n=3$-line, another …
Ionization energies for Rydberg $^4 \mathrm{He}$ ($1snp\,^{1,3}P$) states using the correlated B-spline basis function method
Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences（中国科学院精密测量科学与技术创新院）；University of Chinese Academy of Sciences（中国科学院大学）
